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Tucci will play Dr. Abraham Erskine, who in the Marvel Comics series was a scientist behind a super-soldier program that gave the title hero his powers.
Due in theaters July 22, 2011, "Captain America" stars Chris Evans in the title role and also features Hugo Weaving and Hayley Atwell.
Tucci, whose credits include "The Devil Wears Prada" and "Julie&Julia," earned a supporting-actor nomination at the Oscars for last year's "The Lovely Bones."
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